Relationship between cyclic tensile properties of cellulose nanofiber reinforced natural rubber and volume fraction of bound rubber obtained from swelling tests

In recent years, environmental concerns have led to a demand for sustainable materials, and natural rubber (NR) reinforced with cellulose nanofibers (CNFs) has been attracting attention as one such material. When CNFs are added to NR, the elastic modulus is greatly improved. This is considered to be caused by deformation constraint of NR by reinforcing CNFs. On the other hand, it is known that there exists a region around reinforcing fibers where the rubber is tightly connected to the surface of fibers, which is called bound rubber. The volume fraction of the bound rubber is usually measured by swelling tests using organic solvent. In this paper, we focused on the relationship between the tensile properties of NR reinforced with CNFs and the volume fraction of bound rubber. Firstly, cyclic tensile tests were performed using plate specimens of CNF-reinforced NR and the effect of reinforcing CNFs on the tensile properties of CNF-reinforced NR and their change with loading cycles were investigated. Then, the swelling tests were conducted for similar specimens and the volume fraction of the bound rubber was evaluated. It was found from a series of experimental results that tensile deformation resistance of NR increased largely by adding 5 phr (4.8 mass%, 3.2 vol.%) of CNFs but that this increase decreased from the second loading cycle. Moreover, a clear relationship was found between the tensile deformation resistance of CNF-reinforced NR and the volume fraction of bound rubber. These results suggest that the tensile deformation resistance of CNF-reinforced NR can be evaluated by swelling tests.